Solution-processed semiconducting carbon nanotube transistors with a high mobility and an ON/OFF ratio are the most promising for use in flexible electronics. In this paper, we report low-k/high-k bilayer polymer dielectrics for solution-processed semiconducting single-walled carbon nanotube (s-SWNT) field-effect transistors (s-SWNT-FETs) with efficient charge transport and operation at low voltage. Thin low-k polystyrene (10 nm) is used for the first contact insulator with a channel in order to passivate the dipolar disorder induced by high-k insulators. The second gate insulator for low voltage operation is cyanoethyl pullulan (CEP), which is an environmentally friendly high-k insulator based on cellulose. Moreover, poly[(vinylidenefluoride-co-trifluoroethylene) is chosen as a single layer dielectric for comparison. A reasonably low operational voltage (<10 V) and high operational stability are achieved by the s-SWNT-FETs with polystyrene/CEP bilayer gate dielectrics. In addition, this indicates that the interface between the s-SWNTs and the low-k insulator is of critical importance for efficient charge transport.